Process for production of laminated film having reduced neck-in-forming property

ABSTRACT

A process for the production of laminated film which comprises extruding from an extruder die a melted resin having a high neckin-forming property together with another melted resin having a lower neck-in-forming property, then laminating the extruded resin in the form of a melted compounded film with a base material.

United States Patent Inventors Kohei Masuda;

Taku Uchigaki; Masakazu Arai, all of Yokkaichi-shi, Japan Appl. No. 702,087

Filed Jan. 31,1968

Patented Dec. 21, 1971 Assignee Mitsubishi Petrochemical Co., Ltd.

Tokyo, Japan Priority Jan. 31,1967

Japan 42/5968 PROCESS FOR PRODUCTION OF LAMINATED FILM HAVING REDUCED NECK-IN-FORMING PROPERTY 6 Claims, 8 Drawing Figs.

U.S. Cl [56/244, 156/306, 117/72 Int. Cl B29c 19/00 Field of Search 156/244,

[56] References Cited UNITED STATES PATENTS 2,932,323 4/1960 Aries 156/244 X 3,046,155 7/1962 Reinke 156/244 X 3,161,560 12/1964 Paquin et al. 156/244 X 3,190,781 6/1965 Metz 156/244 3,196,063 7/1965 Paquin et a1. 156/244 X 3,230,126 1/1966 Craver 156/244 3,341,388 9/1967 Bunyea..... 156/244 3,371,002 2/1968 Reddeman 156/244 3,416,986 12/1968 Carley 156/244 3,418,396 12/1968 Edwards et a1. 156/244 X 3,448,000 6/1969 Paquin et a1. 156/244 X Primary Examiner-Carl D, Quariorth Assistant Examiner-Stephen J. Lcchert. Jr. Art0rney-Su ghrue, Rothwell, Mion, Zinn & Mucpeuk ABSTRACT: A process for the production of laminated film which comprises extruding from an extruder die a melted resin having a high neck-in-forming property together with another melted resin having a lower neck-in-forming property, then laminating the extruded resin in the form of a melted compounded film with a base material.

PATENIEllllttzllm 3529 03 SHEET 1 OF 2 FIG. 4

INVENTORS' KOHEI MASUDA TAKU UCHlGAKl MASAKAZU ARA! BY $14 M, lemma, r j/M, Zw y Ma m ATTORNEYS PATENTEI] 115221 1971 31629037 SHEET 2 [IF 2 H66 FIG? H08 PROCESS FOR PRODUCTION OF LAMINATED FILM HAVING REDUCED NECK-IN-FORMING PROPERTY BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a process for the production of laminated film by the extrusion-laminating of thermoplastic resins. More particularly, it relates to a process for the production of laminated film having reduced neck-informing properties.

2. Description of the Prior Art In general, laminated film is produced by the use of such a conventional type extrusion-laminating apparatus as described in FIG. I, which apparatus comprises extruder 1, die 2 fitted to extruder l, and press rolls consisting of pinch roll 3 and metal roll 4 in pairs. In conducting the lamination of a thermoplastic resin with a base material, such as paper and cellophane, resin film b extruded from manifold 5 of die 2 through slit 6 is still maintained in the melted state, so that the extruded resin film b which has once come out of the slit in the slit width of W of die 2 shrinks widthwise by the action of surface tension into a width W when it is about to be laminated with the base material by pressure between pinch roll 3 and metal roll 4. Both edges cc of the resin film b will come to have a thickness more than several times greater than that of other portions as seen in FIG. 3 and FIG. 4 in which the cross section is shown on the line IV-IV in FIG. 3. This phenomenon is known as neck-in" and results in the considerable loss of product material because these thickened edges must be cut off as waste in order to give a product of uniform thickness. Moreover, the film having such thickened edges often tends to stick on and wind around the press roll since thicker edges cc have greater heat capacity and hence give rise to less temperature loss during working than that of other portions.

The neck-in troubles are especially significant when polypropylene or high-density polyethylene is used as the thermoplastic resin, and the use of such resins is much more uneconomical in terms of product yield than other resins having relatively less neck-in-forming properties, such as low-density polyethylene. Thus, the characteristic features of polypropylene and high-density polyethylene have not been sufficiently utilized in the field of extrusion lamination.

The object of this invention is to provide laminated film having reduced neck-in-forming properties. Another object of this invention is to eliminate the troubles of the sticking of the film to the press rolls due to thickened edges.

SUMMARY OF THE INVENTION The process of this invention comprises compounding a resin of high neck-in-forming property, e.g. polypropylene and high-density polyethylene, with a resin of lower neck-in-forming property; both resins may be of the same kind, in the melted state, then press-laminating a base material with the compounded film-shaped resin. More particularly, the process comprises separately pouring down the melted resin of high neck-in-forming property and the melted resin of lower neckin-forming property each from the slit in the extruder die, combining both melted flows and extruding as a melted compounded film, then press-laminating with the base material. In another embodiment of the process of this invention, the melted resin of higher neck-in-forming property and the melted resin of lower neck-in-forming property are separately extruded from the slits of the extruder die, and they are combined at the location just below the outlet of each slit into a melted compounded film and then laminated with the base material thereby to reduce neck-in to a great extent.

BRIEF DESCRIPTION OF THE DRAWINGS A better understanding of the present invention will be attained from a review of the drawings accompanying the present application, in which:

FIG. I represents a conventional type extrusion-laminating apparatus;

FIG. 2 represents a conventional type extruder die;

FIG. 3 represents a resin film exhibiting neck-in" properties;

FIG. 4 is a cross section of FIG. 3;

FIGS. 5 and 6 represent an extrusion die for carrying out the process of the present invention;

FIG. 7 represents a die having three separated manifolds with communicating slits and an inner joint at which melted resin flows may be combined; and

FIG. 8 is a die having separated manifolds with communicating slits ending at separated orifice outlets whereby melted resin flows may be combined at the place directly beneath the outlets.

DETAILED DESCRIPTION OF THE INVENTION The operation of the process of this invention will be more fully explained in reference to the attached drawings of FIG. 5 and 6.

Die 7 to be fitted to the extruder has slit 9 connected to manifold 8 and slit ll connected to manifold 10 as shown in FIG. 6. Both slits are combined together at junction I3 in front of outlet orifice 12. There is also provided a parallel passage 14 between'outlet I2 and junction 13, said passage 14 having a gap size of the total of the gaps of slit 9 and slit II. Melted resin d having greater neck-in-forming property is allowed to flow down from manifold 8 through slit 9, and melted resin e having lower neck-in-forming property is passed from manifold 10 through slit 1]. Both melted flows are combined at junction 13 and passed through parallel line 14, then finally extruded at orifice outlet 12 as melted compounded film f.

By operating in this way, a laminated film is formed having much more uniform thickness than those obtained in the conventional processes wherein a resin of high neck-in-forming property is extruded alone into film shape and laminated with a basic material. In other words, it is possible to reduce neckin and hence to improve the product yield to a remarkable extent.

The extruder die to be used in the process of this invention may be designed in a variety of modified types other than as shown in FIG. 6.

In one example, it may be made into die 18 having three separated manifolds I5, 16 and 17 each connected to slits l5, l6 and I7, and having an inner joint at which melted resin flows are combined together, as illustrated in FIG. 7. In another example, die 2] may have separated manifolds l9 and 20 each connected to slits l9 and 20' ending at separated orifice outlets 19" and 20", and the melted resin flows are combined together at the place directly beneath the outlets l9" and 20", as illustrated in FIG. 8.

The degree of neck-in-forming property is not only defined as to resins of different kinds, but also defined according to the value of specific gravity in the same resin. For instance, the resin having higher specific gravity exhibits increased neck-in-forming property and the resin with lower specific gravity shows lower neck-in-forming property. The neck-informing property is also affected by the extrusion tempera-v ture, even in using a resin of the same kind and of the same specific gravity. Usually, those extruded at higher temperature will have increased neck-in-forming property, whereas those extruded at lower temperature will have a lower neck-in-forming property. It is, therefore, possible to prepare a compounded film consisting of the same resin in which the one is extruded at a higher temperature and the other is extruded at a lower temperature.

A number of combinations between the resins having higher neck-in-forming property and the resins having lower neck-informing property may be used in the practice of the present invention. Examples of the former type resins include polypropylene, mediumand low-pressure polyethylenes, high-pressure polyethylene having relatively high specific gravity, etc. The latter type resins typically include high-pressure polyethylene having relatively low-specific gravity.

Examples of the combination of resins in the compounded film to be used in accordance with the process of this invention are polypropylene/lowdensity polyethylene/substrate, high-density polyethylene/low-density polyethylene/substrate, polyester/low-density polyethylene/substrate, polyvinylidene chloride/low-density polyethylene/substrate and the like.

according to the process of this invention, from manifold ll and slit 9 together with ethylene-vinyl acetate copolymer, made by Mitsubishi Petrochemical Co. Ltd, extruded separately from manifold 10 and slit ll, to form melted com- Even using resins of the same kind, the combination of highpounded film f which was thereafter laminated with craft temperature extrusion of high neck-in-forming property with paper a. The results ofthese tests are given in table I. low-temperature extrusion of lower neck-informing property The tests were carried out according to the following data: may be possible and attain excellent adhesion at a high-tem- Tests No. l and No. 2 (Conventional Process) perature extrusion side as well as reduction in the neck-in- Extruder: Diameter=2$ inches, length/diameter=24 forming property at the low-temperature extrusion side by Die: Slit width=600 mrn. selecting the high-temperature extrusion side as the adhesion Air Gap (distance between die and press roll): 75 mm. side with the matrix surface. Extrusion Rate: 600 g./min.

Two types of resins each differing in the neck-in-forming Winding Speed: 40 m./min. property may be applied on either side to the basic material, Tests No. 3 and No. 4 (Process of this Invention) i.e., they may be: laminated with the basic material either in- Extruder:

side or outside the basic material. The neck-in-forming pro- ForiDiameter=2 inches, lengthldiameter=24 petty will not be influenced in either case including the case For ii Diameter=40 mm. lengthldiameter= 24 where the resin of high neck-imforming property is interposed Die: The type used was as shown in FIG. 6

between the basic material and the resin of lower neck-in- Fort'Slit width=600 mm.

forming property, or where it is laminated outside the resin of For ii Slit width 600 mm.

lower neck-in-forming property with respect to the basic The Su r e a wa hered a h ide of layer ii. material. Therefore, the determination of which resin in the l' P 75 mmtwo layers should be applied inside or outside the basic materii H 2 al can be made according to such conditions as the strength of YP PYI 400 gJ adhesion between the basic material and the resin surface, the E hyl n nyl acetate copolymer 200 gJ property required as a compounded film (e.g., heat sealing winding Speed: 40 -lminro t a d th lik Tests No. 5 and No. 6 (Process of this Invention) In accordance with the process of this invention, it is possi- The working Conditions were the Same as 16818 NO. 3 and ble to improve the product yield to a great extent and also 4 l" as follows: possible to conduct the resin heating at a possibly lower tem- Di perature, as long as good adhesion can be maintained in the ForiSlit Width=600 mm. production of laminated film wherein the characteristic fea- For ii SlitWidth=608 mm. tures of the resin having high neck-in-forming property is ad (The width of slit for ii was extended towards both sides vantageously utilized. Moreover, it is also possible to eliminate each 4 mm. wider than that of slit for i) TABLE 1 Neck, in mm. Working c- Processes Test No. Resins temp, Substrate Wl-Wg W1-W3 Adh i Conventional sap py 300 Craft paper 1 180 Good 0 .i 260 .....(10 10 125 Bad.

3 o yp opyl 300 do 30 Good.

Ethylene-vinyl acetate copolymer (ll) 300 4 {Polypropylene (i). 60 }...d0 v. 25 35 Do. This invention Ethylene-vinyl acetate copolymer (1l) 300 5 ggttzlly iropylene (i) 300 iguhdo 27 36 Do.

y ene-vlnyl acetate copolymer (ii) 300 6 {Polypropylene (i) 260 }....do 23 30 Do.

Ethylene-vinyl acetate copoly'mer (ll) 300 EXAMPLE 2 the trouble in the winding step due to neck-in because the neck-in is greatly reduced so as to produce laminated film having uniform thickness over wide areas. Other advantages of the process of this invention will be apparent from the description of examples set forth below.

EXAMPLE 1 The lamination according to the process of this invention was carried out by using polypropylene made by Mitsubishi Petrochemical Co., Ltd. (melt index 20, isotactic index 95) as a laminating resin and craft paper as the substrate. For the comparison, polypropylene alone is extruded by using a conventional-type extruder die as shown in FIG. 2 and laminated with craft paper a. Polypropylene is also extruded The process of this invention was applied to the same resin having a different specific gravity and the results were as follows:

ln carrying out the extrusion-lamination of polyethylene (made by Mitsubishi Petrochemical Co. Ltd., Melt Index 4, Specific Gravity 0.930) with usual cellophane, polyethylene ii alone was extruded from a conventional extrusion die 2 of the type shown in FlG. 2, and it was also extruded according to the process of this invention from die 2] through manifold 20, slit 20' and outlet orifice 21" together with another polyethylene (made by Mitsubishi Petrochemical Co. Ltd, Melt index 4, Specific Gravity 0.918) separately extruded from manifold l9, slit 19' and outlet orifice 19", then com bined together directly below each outlet orifice 19', 20 into melted compounded film and laminated with cellophane a. The results of these tests are given in table 2 below.

TABLE 2 Working Neck, in mm.

temp. Process Test No. Rosin C. Substrate Wl-Wfl W Wl Adhesion i 7 lKEtil) 310 Cellophane. 65 Good. comemlmal "l s Ratio 280 i.... 1 so so Bad.

1) 1.E.(il 310 v m PEIUV) 310 do Z7 40 (d. This invention ,i t

280 i do "a 30 Do l.E.(lv) 3101"" Tests in table 2 were carried out under the following conditions:

Tests No. 7 and No. 8 were conducted under the same condition as tests No. l and No. 2 in example i with the ex- What is la m caption f h ki temperature. 5 a. heating a thermoplastic resin normally subject to neck-in Tests Nos. 9 and 10 were conducted under the same condifor tion as extruding said resin into a film and,

Tests 3 and a 1 F fi c. coating said film, while molten, onto said substrate, the wor mg tempfra tare an rate 0 extrusion. ll'a I l 0 improvement which comprises essentially eliminating exlruslo" oye was 400 'f' as to poly y ene said neck-in formation by, in step (b), simultaneously exand 200 as to polyethylene truding a thermoplastic resin layer less subject to neck-in EXAMPLE 3 formation together with said thermoplastic resin to form a multilayer thermoplastic film which is coated onto said in carrying out extrusion-lamination of usual cellophane l5 substrate in accordance with step (c).

polyethyle? (made y phlu'ps Pe tr]eum P" 2. The process of claim 1 wherein different thermoplastic speclfic Gravny 0958) the Pests w G resins are employed in the formation of said multilayer therout in two manners for the sake of comparison, in which the mophstic m one comprised the extrusion of the above polyethylene alone from a conventional-type extruder die of the type shown in T Process clam l wherem the Same thermoplasuc FIG. 2, and the other was effected according to the process of employftd m |east tw of the layer? of the mumlayer this invention by extruding above Polyethybne d from plastic film, said layers being formed at different extrusion manifold 8 together with low-density polyethylene e (made by temperatures Mitsubishi Yuka Co. Ltd., Melt Index 4, Specific Gravity 4. The process of claim 1 wherein the thermoplastic resin 0.918) from manifold 10 by using an extruder die 7 of the type normally subject to neck-in formation is selected from the as shown in FIG. 6. group consisting of polypropylene, medium-pressure The results of the tests are given in table 3 below; 7 H polyethylene, low-pressure polyethylene, high-pressure TABLE 3 w k Neck, in mm.

01' ll] Process temp., Substrate W W W W3 Adhesion 310 Cello hane 80 110 Good.

Cmvenmml 280 ma 65 37 Bad.

}Cellophane 31 45 Good. This invention 280 310 do 26 40 Do.

N0m.P.E.=polyethylene, M.I.=melti-ng index, S.G.=specific gravity. Conditions employed in these tests were the same as EXAMPLE 4 In carrying out the extrusion-lamination of substrate craft paper a with polyethylene (made by Mitsubishi Petrochemical Co. Ltd., Melt index 4, Specific Gravity 0.924), experiments were carried out according to two manners in which the one comprised the extrusion of polyethylene v alone at 3l0. C., and lamination with matrix a with the use of a conventional extruder die 2 of the type shown in FIG. 2, and the other was conducted according to the process of this invention by extruding the above polyethylene v at 280 C., from slit 9 of die 7 shown in FIG. 6 together with the extrusion of the same polyethylene v at 310 C. The results are given in table 4 in which test No. 15 was conducted under the same conditions as described in tests Nos. 1 and 2 in example i with the exception of working temperature, and test No. 16 was conducted under the same conditions as tests Nos. 3 and 4 with the exception of the working temperature.

5. The process of claim 1 wherein simultaneous extrusion is accomplished by combining separate resin streams and extruding said combined stream from a single outlet orifice.

6. The process of claim 1 wherein simultaneous extrusion is achieved by extruding each resin stream separately from separate slits in the extrusion dye and combining said separate streams at a point immediately below the outlet orifice of each slit to form the multilayer thermoplastic film.

TABLE 4 Neck, in mm. Test Temp, Process No. Resin C. Substrate W1W W1 W3 Adhesion Conventional 15 P.E. (v) 310 Kraft paper 30 50 Good. This invention.. 16 {1 25 40 Do. 

2. The process of claim 1 wherein different thermoplastic resins are employed in the formation of said multilayer thermoplastic film.
 3. The process of claim 1 wherein the same thermoplastic resin is employed in at least two of the layers of the multilayer plastic film, said layers being formed at different extrusion temperatures.
 4. The process of claim 1 wherein the thermoplastic resin normally subject to neck-in formation is selected from the group consisting of polypropylene, medium-pressure polyethylene, low-pressure polyethylene, high-pressure polyethylene possessing a relatively high specific gravity, polyester and polyvinylidene chloride and the thermoplastic resin layer less subject to neck-in formation comprises a resin selected from the group consisting of high-pressure polyethylene and a copolymer of ethylene with vinyl acetate.
 5. The process of claim 1 wherein simultaneous extrusion is accomplished by combining separate resin streams and extruding said combined stream from a single outlet orifice.
 6. The process of claim 1 wherein simultaneous extrusion is achieved by extruding each resin stream separately from separate slits in the extrusion dye and combining said separate streams at a point immediately below the outlet orifice of each slit to form the multilayer thermoplastic film. 